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研究生:陳勇志
研究生(外文):Chen, Yung-Chih
論文名稱:磁性之幾丁聚醣-檸檬酸凝膠顆粒的合成與應用
論文名稱(外文):Synthesis and application of mangnetic a chitosan-citrate gel beads
指導教授:吳紹榮吳紹榮引用關係
指導教授(外文):Wu, Shao-Jung
口試委員:糜福龍余淑惠
口試委員(外文):Mei, Fu-LungYu, Shu-Hui
口試日期:2012-07-06
學位類別:碩士
校院名稱:明志科技大學
系所名稱:化學工程研究所
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2012
畢業學年度:100
語文別:中文
論文頁數:92
中文關鍵詞:幾丁聚醣磁性奈米粒子檸檬酸吸附
外文關鍵詞:chitosanmagneticnanoparticlescitrateadsorption
相關次數:
  • 被引用被引用:0
  • 點閱點閱:301
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  • 下載下載:10
  • 收藏至我的研究室書目清單書目收藏:0
本研究以製備磁性幾丁聚醣-檸檬酸顆粒對重金屬(銅、汞)離子進行吸附實驗。係先將幾丁聚醣進行羧甲基化反應,藉由碳二醯胺活化直接共價鍵結在磁性四氧化三鐵奈米粒子上,之後添加到幾丁聚醣-檸檬酸溶液內,經由蠕動幫浦滴入氫氧化鈉使其成凝膠顆粒。由XRD分析可得知製備的磁性奈米顆粒為四氧化三鐵之尖晶石結構,而不會因羧甲基幾丁聚醣被覆造成結晶相之改變,並以TEM來觀察磁性奈米顆粒的粒子形狀、粒徑分佈和利用SEM探討所製備顆粒的結構變化,由SQUID測量其磁性性質可得磁性奈米粒子具有超順磁,磁性奈米粒子的飽和磁化量(Ms)、殘留磁化量(Mr)與保磁力(Hc)分別為73.89 emu/g、0.95 emu/g與6.9 Oe,使用FTIR探討其磁性奈米顆粒以及羧甲基幾丁聚醣被覆磁性奈米顆粒官能基的變化。在磁性幾丁聚醣-檸檬酸顆粒之吸附效果分析上,利用等溫吸附模式、吸附動力學模式來進行分析,並且探討吸附熱力學ΔH°、ΔG°和ΔS°的變化。
This study used an in-liquid curing method by the ionotropic crosslinking with nontoxic citric acid to synthesize the chitosan-citrate beads, which are used to fabricate magnetic chitosan beads. The magnetic chitosan-coated iron oxide nanoparticles have been synthesized from carboxymethyl chitosan with covalently bonded on the surface of iron oxide nanoparticles via carbodiimide activation. The magnetic chitosan-coated Fe3O4 nanoparticles (MNPs) were dispersed in chitosan-citrate beads, and were thus able to maintain appropriate dispersion and stability, which greatly improves their applicability. The characterization of magnetic nanoparticles and magnetic chitosan-citrate beads were investigated by means of FTIR, X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), superconductive quantum interference devices (SQUID). The present study aims to explore the adsorption capacities, kinetics and thermodynamics of metal ions from aqueous solution onto fabricated magnetic gelled beads. The effects of the initial pH value of the solution, contact time and the initial metal ion concentration on the adsorption of metal ion were investigated. The adsorption data of Cu(II) ion obeyed the Freundlich equation and Hg(II) ion obeyed the Langmuir equation. The adsorption kinetics were well described by the pseudo-second order equation, indicating that chemical adsorption is the rate-limiting step for the adsorbents. The thermodynamic parameters such as enthalpy change(ΔH°), entropy change (ΔS°)and Gibbs free energy change(ΔG°) were computed and the results showed that the adsorption of Cu(II) ion onto chitosan-citrate beads was spontaneous and exothermic and Hg(II) ion onto chitosan-citrate beads was spontaneous and endothermic in nature.
明志科技大學碩士學位論文指導教授推薦書 i
明志科技大學碩士學位論文口試委員會審定書 ii
明志科技大學學位論文授權書 iii
誌謝 iv
中文摘要 v
Abstract vi
目錄 viii
表目錄 xii
圖目錄 xiii
第一章 緒論 1
1-1 研究動機 1
1-2 研究項目 2
1-2-1 吸附劑製程 2
1-2-2 特性分析 2
1-2-3 吸附劑吸附行為探討 2
第二章 文獻回顧 3
2-1 幾丁聚醣 3
2-1-1 幾丁聚醣簡介 3
2-1-2 幾丁聚醣之特性 5
2-1-3 幾丁聚醣吸附重金屬之特性 7
2-1-4 幾丁聚醣之應用 8
2-2 奈米材料與科技 11
2-2-1 奈米之簡介 11
2-2-2 奈米材料特性 12
2-2-3 奈米材料之製備 14
2-3 磁性理論 15
2-3-1 超順磁性 15
2-3-2 磁滯曲線 17
2-3-3 磁性奈米粒子簡介 20
2-3-4 四氧化三鐵之應用 21
2-4 銅的特性與危害 23
2-5 汞的基本性質與危害 26
2-5-1 汞的來源 26
2-5-2 汞的基本性質 27
2-5-3 汞的危害 28
2-6 吸附理論 30
2-7 等溫吸附模式 32
2-8 動力學吸附模式 34
2-9 熱力學吸附模式 37
第三章 實驗方法與設備 38
3-1 實驗藥品 38
3-2 實驗設備與分析儀器 40
3-3 羧甲基幾丁聚醣被覆磁性奈米粒子之製備 42
3-3-1 四氧化三鐵(Fe3O4)磁性奈米微粒之製備 42
3-3-2 羧甲基化幾丁聚醣之製備 42
3-3-3 羧甲基幾丁聚醣被覆磁性奈米粒子之製備 43
3-4 吸附劑之製備 44
3-5 吸附劑吸附銅離子溶液之吸附實驗 45
3-5-1 不同pH值吸附實驗 45
3-5-2 等溫吸附實驗 46
3-5-3 動力學吸附探討 48
3-5-4 不同溫度吸附探討 48
3-6 吸附劑吸附汞離子溶液之吸附實驗 49
3-6-1 不同pH值吸附實驗 49
3-6-2 等溫吸附實驗 50
3-6-3 動力學吸附探討 52
3-6-4 不同溫度吸附探討 52
3-7 XRD分析 53
3-8 DLS分析 53
3-9 TEM分析 54
3-10 FTIR分析 54
3-11 SQUID分析 54
3-12 TGA分析 55
3-13 SEM分析 55
3-14 金屬離子溶液分析 55
第四章 結果與討論 56
4-1 XRD分析 56
4-2 DLS分析 57
4-3 TEM分析 58
4-4 FT-IR分析 59
4-5 SEM分析 61
4-6 SQUID分析 66
4-7 TGA分析 68
4-8 吸附劑的製作 69
4-9 pH值對吸附的影響 70
4-10 等溫吸附模式探討 72
4-11 動力學吸附探討 76
4-12 熱力學吸附探討 83
第五章 結論 85
第六章 參考文獻 87
1.Kurita, K., Controlled functionalization of the polysaccharide chitin. Progress in Polymer Science 2001, 26 (9), 1921-1971.
2.蔡家樺. 幾丁聚醣摻合PU基材之物性及抑菌研究。中央大學,桃園,2003。
3.楊惠嘉. 利用幾丁聚醣吸附卡馬西藍染料之研究。成功大學,臺南,2003。
4.王嘉薇. 丁醯化幾丁聚醣之研究。成功大學,臺南,2003。
5.Ng, J.C.Y.; Cheung, W.H.; McKay, G., Equilibrium Studies of the Sorption of Cu(II) Ions onto Chitosan. Journal of Colloid and Interface Science 2002, 255 (1), 64-74.
6.Chang , M.Y.; Juang, R. S., Adsorption of tannic acid, humic acid, and dyes from water using the composite of chitosan and activated clay. Journal of Colloid and Interface Science 2004, 278 (1), 18–25.
7.Domard, A.; Rinaudo, M.; Preparation and characterization of fully deacetylated chitosan. International Journal of Biological Macromolecules 1983, 5 (1), 49-52.
8.Miyazaki, S., Chitin and chitosan as vehicle for drug delivery. Zairyo Gijutsu 1998, 16, 276.
9.Ritthidej, G. C.; Chomto, P.; Pummangura, S.; Menasveta, P., Chitin and chitosan as disintegrants in paracetamol tablets. Drug Development and Industrial Pharmacy 1994, 20 (13), 2019-2134.
10.Calvo, P.; Remunan-Lopez, C.; Vila-Jato, J. L.; Alonso, M.J., Novel hydrophilic chitosan-polyethylene oxide nanoparticles as protein carriers. Journal of Applied Polymer Science 1997, 63 (1), 125-132.
11.Kratz, G.; Back, M.; Arnander, C.; Larm, O., Immobilised Heparin Accelerates the Healing of Human Wounds In Vivo. Scandinavian Journal Plastic and Reconstructive Surgery and Hand Surgery 1998, 32 (4), 381-386.
12.范恆誠. 應用幾丁質在幾種飲料中澄清作用的研究。食品科學期,1991,12 (7),30- 36。
13.Young, D. H.; Kohle, H.; Kauss, H., Effect of chitosan on membrane permeability of suspension-cultured Glycine max and Phaseolus vulgaris cells. Plant Physiology 1982, 70 (5), 1449-1454.
14.Knorr, D., Functional properties of chitin and chitosan. Journal of Food Science 1982, 47 (2), 593-595.
15.Sharma, S. C., Gum and hydrocollids in oil-water emulsions. Food Technology 1981, 35, 59-63.
16.Chen, A. H.; Liu, S. C.; Chen, C. Y.; Chen, C. Y., Comparative adsorption of Cu(II), Zn(II), and Pb(II) ions in aqueous solution on the crosslinked chitosan with epichlorohydrin. Journal of Hazardous Materials 2008, 154 (1-3), 184–191.
17.吳彰哲,黃瀚寧. 蝦蟹殼中的寶貝–幾丁質。科學發展,2010,448, 12-19。
18.Aly, A. S.; Jeon, B. D.; Park, Y. H., Preparation and evaluation of the chitin derivatives for wastewater treatments. 1997, John Wiley & Sons Incorporated, 1939-1946.
19.Majeti, N. V.; Ravi, K., A review of chitin and chitosan applications. Reactive and Functional Polymers 2000, 46 (1), 1-27.
20.黃德歡 (2002)。改變世界的納米技術;瀛舟出版社。
21.張立德,牟季美 (2002)。奈米材料與奈米結構;滄海書局。
22.尹邦躍 (2002)。奈米時代;五南圖書出版股份有限公司。
23.吳國卿,董玉蘭. 奈米粒子的基本特性。化工資訊月刊,1999,42-46。
24.張志焜,崔作林 (2000)。納米技術與納米材料 ;北京國防工業出版社。
25.廖敏宏. 磁性奈米載體在生物觸媒和生化分離之應用。成功大學,臺南,2002。
26.王世敏,許祖勛,傅晶 (2004)。奈米材料原理與製備;五南圖書出版股份有限公司。
27.鄭豐裕. 四氧化三鐵磁性奈米粒子之製備及其在生物醫學上之應用。成功大學,臺南 2006。
28.黃忠良 (1989)。磁性流體理論應用;復漢出版社。
29.Sen, T.; Sebastianelli, A.; Bruce, I.J., Mesoporous Silica-Magnetite Nanocomposite: Fabrication and Applications in Magnetic Bioseparations. Journal of the American Chemical Society 2006, 128 (22), 7130-7131.
30.Ohe, K.; Tagai, Y.; Nakamura, S.; Oshima, T.; Baba, Y., Adsorption Behavior of Arsenic(III) and Arsenic(V) Using Magnetite. Journal of Chemical Engineering of Japan 2005, 38 (8), 671-676.
31.馮端 (1998)。固態物理學大辭典;建宏出版社。
32.Cullity, B.D.; Graham, C. D., Introduction to Magnetic Materials. 1984, John Wiley & Sons Inc.
33.關曉輝,趙潔,秦玉春. 納米Fe3O4的製備及其輔助吸附重金屬離子的特性。環境化學,2005,24 (4),409-412。
34.Tourinho, F.; Franck, R.; Massart, R., Aqueous ferrofluids based on manganese and cobalt ferrites. Journal of Materials Science 1990, 25 (7), 3249-3254.
35.Tourinho, F.; Franck, R.; Massart, R.; Perzynski, R., synthesis and magnetic properties of manganese and cobalt ferrite ferrite ferrofluids. Progress in Colloid and Polymer Science 1989, 78, 128-134.
36.Chang, Y.C.; Chen, D.H., Preparation and Adsorption Properties of Monodisperse Chitosan-Bound Fe3O4 Magnetic Nanoparticles for Removal of Cu(II) Ions. Journal of Colloid and Interface Science 2005, 283 (2), 446-451.
37.Zhao F.; Yu B.; Yue Z.; Wang T.; Wen X.; Liu Z.; Zhao C., Preparation of porous chitosan gel beads for copper(II) ion adsorption. Journal of Hazardous Materials 2007, 147 (1-2), 67-73.
38.Aly, S.A.; Jeon, B.D.; Park, Y.H., Preparation and Evaluation of the Chitin Derivatives for Wastewater Treatments. Journal of Applied Polymer Science 1997, 65 (10), 1939-1946.
39.Kim, C.Y.; Choi, H.M.; Cho, H.T., Effect of Deacetylation on Sorption of Dyes and Chromium on chitin. Journal of Applied Polymer Science 1997, 63 (6), 725-736.
40.Peter, M.G., Applications and Environmental Aspects of chitin and Chitosan. Journal of Macromolecular Science Pure and. Applied Chemistry 1995, A32 (4), 629-640.
41.Huang, C.; Chung, Y.C.; Liou, M.R., Adsorption of Cu(II) and Ni(II) by pelletized biopolymer. Journal of Hazardous Materials 1996, 45 (2-3), 265-277.
42.NG, J.C.Y.; Cheung, W.H.; Nckay, G., Equilibrium studies for the sorption of lead from effluents using chitosan. Chemosphere 2003, 52 (6), 1021-1030.
43.Coelho, T.C.; Laus, R.; Mangrich, A.; de Favere, Valfredo T.; Laranjeira, Mauro C.M., Effect of heparin coating on epichlorohydrin cross-linked chitosan microspheres on the adsorption of copper(II) ions. Reactive and Functional Polymers, 2007, 67 (5), 468-475.
44.Vasconcelos, H. L.; Favere, V. T.; Goncalves, N. S.; Laranjeira, Mauro C.M., Chitosan modified with Reactive Blue 2 dye on adsorption equilibrium of Cu(II) and Ni(II) ions.” Reactive and Functional Polymers, 2007, 67 (10), 1052-1060.
45.Vasconcelos, H.; Guibal, L.; Laus, E. R.; Vitali, L.; Favere, V. T. , Competitive adsorption of Cu(II) and Cd(II) ions on spray-dried chitosan loaded with Reactive Orange 16. Materials Science and Engineering: C, 2009, 29 (2), 613-618.
46.Popuri, S. R.; Vijaya, Y.; Boddu, V.M.; Abburi, K., Adsorptive removal of copper and nickel ions from water using chitosan coated PVC beads. Biochemical Technology 2009, 100 (1), 194-199.
47.Ngah, W.S.; Fatinathan, S., Adsorption characterization of Pb(II) and Cu(II) ions onto chitosan-tripolyphosphate beads: Kinetic, equilibrium and thermodynamic studies. Journal of Environmental Management 2010, 91 (4), 958-969.
48.Ngah, W.S.; Fatinathan, S., Adsorption of Cu(II) ions in aqueous solution using chitosan beads,chitosan–GLA beads and chitosan–alginate beads. Chemical Engineering Journal 2008, 143 (1-3), 62-72.
49.Justi, K.C.; Fávere, V.T.; Laranjeira, M.C.; Neves, A.; Peralta, R.A., Kinetics and equilibrium adsorption of Cu(II), Cd(II), and Ni(II) ions by chitosan functionalized with 2[-bis-(pyridylmethyl)aminomethyl]-4-methyl-6-formylphenol. Journal of Colloid and Interface Science 2005, 291 (2), 369-374.
50.Kannamba, B.; Reddy, K.L.; AppaRao. B.V., Removal of Cu(II) from aqueous solutions using chemically modified chitosan. Journal of Hazardous Materials 2010, 175 (1-3), 939–948.
51.Gyliene, O.; Binkiene, R.; Butkiene, R., Sorption of Cu(II) complexes with ligands tartrate, glycine and quadrol by chitosan. Journal of Hazardous Materials 2009, 171 (1-3), 133–139
52.張榮傑. 以檸檬酸與蘋果酸改質幾丁聚醣之製備與分析。明志科技大學,臺北,2011。
53.洪東良. 多孔性幾丁聚醣螯合型樹脂之合成與應用。明志科技大學,臺北,2010。
54.Lange, N.A., Handbook of Chemistry. 1976, McGraw-Hill, 288-290.
55.Li, N.; Bai, R., Development of chitosan-based granular adsorbents for enhanced and selective adsorption performance in heavy metal removal. Water Science and Technology 2006, 54 (10), 103–113.
56.Genc, O.; Soysal, L.; Bayramoglu, G.; Arica, M.Y.; Bektas, S., Procion Green H-4G immobilized poly (hydroxyethylmethacrylate/chitosan) composite membranes for heavy metal removal. Journal of Hazardous Materials 2003, 97 (1-3), 111–125.
57.Yang, Z.; Yuan, Y.; Wang, Y., Synthesis and evaluation of chitosan aryl azacrown ethers as adsorbents for metal ions. Journal of Applied Polymer Science 2000, 77 (14), 3093–3098.
58.Song, J.; Li, J.; Wang, D.; Wang, Y., Study on crosslinked carboxymethyl chitosan for adsorbing trace inorganic mercury. Ion Exchange Adsorption 2008, 24 (2), 175–182.
59.Monier, M.; Abdel-Latif, D.A., Preparation of cross-linked magnetic chitosan-phenylthiourea resin for adsorption of Hg(II), Cd(II) and Zn(II) ions from aqueous solutions. Journal of Hazardous Materials 2012, 209-210, 240-249.
60.Vieira, R. S.; Beppu, M., Interaction of natural and crosslinked chitosan membranes with Hg(II) ions. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2006, 279 (1-3), 196–207.
61.Jeon, C.; Holl, W.H.H., Chemical modification of chitosan and equilibrium study for mercury ions removal. Water Research 2003, 37 (19), 4770–4780.
62.Zhou, L.-M.; Liu, S.-R.; Huang, Q.-W., Adsorption of mercury and uranyl onto poly(ethyleneimine) grafted chitosan microspheres. Modern Chemical Industry 2007, 27 (179), 175–177.
63.Vieira, R. S.; Beppu, M., Mercury ion recovery using natural and crosslinked chitosan membranes. Adsorption 2005, 11, 731–736.
64.Genc, O.; Arpa, C.; Bayramoglu, G.; Arica, M.Y.; Bektas, S., Selective recovery of mercury by Procion Brown MX 5BR immobilized poly (hydroxyethylmethacrylate/chitosan) composite membranes. Hydrometallurgy 2002, 67 (1-3), 53–62.
65.Cardenas, G.; Parra, O.; Taboada, E., Synthesis and applications of chitosan mercaptanes as heavy metal retention agent. International Journal of Biological Macromolecules 2001, 28 (2), 167–174.
66.Qu, R.; Sun, C.; Ma, F.; Zhang, Y.; Ji, C.; Xu, Q.; Wang, C.; Chen, H., Removal and recovery of Hg(II) from aqueous solution using chitosan-coated cotton fibers. Journal of Hazardous Materials 2009, 167 (1-3), 717-727.
67.Noll K. E., Adsorption technology for air and water pollution control. 1992, Lewis publishers.
68.Langmuir, I., The adsorption of gases on plane surfaces of glass, mica and platinum. Journal of the American Chemical Society 1918, 40 (9), 1361-1403.
69.Freundlich, H.M.F., U¨ ber die adsorption in lo¨sungen. Zeitschrift fur Physikalische Chemie (Leipzig) 1906, 57 (A),385-470.
70.Eagleton, L.C.; Acrivos, A.; Vermeulen, T., Pore and solid-diffusion kinetics in fixed bed adsorption under constant pattern conditions. Industrial & Engineering Chemistry Fundamentals 1966, 5 (2), 212-223.
71.Lagergren, S., Zur theorie der sogenannten adsorption geloester stoffe,Kungliga Svenska Vetenskapsakademiens. Handlingar 1898, 24 (4), 1–39.
72.Ho, Y.S.; McKay, G., The sorption of lead(II) ions on peat. Water Research 1999, 33 (2), 578-584.
73.Ho, Y.S.; McKay, G., Sorption of dye from aqueous solution by peat. Chemical Engineering Journal 1998, 70 (2), 115-124.
74.Singh, K. K.; Rastogi, R.; Hasan, S. H., Removal of Cr(VI) from wastewater using rice bran. Journal of Colloid and Interface Science 2005, 290 (1), 61-68.
75.Ngah, W. S.; Fatinathan, S., Adsorption characterization of Pb(II) and Cu(II) ions onto chitosan-tripolyphosphate beads: Kinetic, equilibrium and thermodynamic studies. Journal of Environmental Management 2010, 91 (4), 958-969.
76.Ho, Y.S.; McKay, G., The kinetics of sorption of divalent metal ions onto sphagnum moss peat. Water Research 2000, 34 (3), 735-743.
77.Weber, W.J. Jr.; Morris, J.C., Kinetics of adsorption on carbon from solution. Journal of the Sanitary Engineering Division 1963, 89 (2), 31-60.
78.Ho, Y.S., Review of second-order models for adsorption systems, Journal of Hazardous Materials 2006, 136 (3), 681-689.
79.Ho, Y.S.; McKay, G., Pseudo-second order model for sorption processes. Process Biochemistry 1999, 34 (5), 451-465.

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1. 丁興祥、陳明穗、蔡啟通、邱皓政、李宗沅(1991)。羅塞浦創造傾向量表修正報告,測驗年刊,38,189-200。
2. 呂燕卿(1999)。簡介九年一貫藝術與人文課程綱要之理念與特色。北縣教育,29,7。
3. 吳明雄、張中一、饒達欽(2008)。高中職學生藝術創造力影響指標之研究:以全國競賽得獎學生為對象。藝術教育研究,16,1-31。
4. 李慧芳(2000)。創造力99解析。設計學報,5(1)。
5. 林小玉(2003)。音樂創造力之內涵與研究趨勢探討。音樂藝術學刊,2,87-118。
6. 林小玉(2005)。邁向藝術課程模式應用於國小五年級學童編曲創作知能之研究。藝術教育研究,10,87-126。
7. 侯禎塘(2010)。創意藝術表達活動於國小美術班學生創造力與情意輔導之研究。特殊教育與輔助科技學報,1,57-79。
8. 洪懿妍(2001)。世界向美走-天下雜誌2001年教育特刊美的學習。台北:天下。
9. 洪久賢、胡夢蕾(2007)。廚藝創造力發展歷程量表之發展研究。教育心理學報,39(3),1-20。
10. 張玉成(1989)。如何有效實施創造思考教學。創造思考教育,創刊號,17-28。
11. 張玉佩(2002)。創造力可以教嗎?談影響創造力發展的相關因素。資優教育季刊,84,22-30。
12. 陳奐宇(2002)。創造力在美術教學上的運用。美育,145,66-79。
13. 陳昭儀(2003)。創意人物研究之回顧與探析。資優教育季刊,87,27-40。
14. 陳昭儀(2006b)。傑出音樂家創作歷程之研究。特殊教育研究學刊,31,221-240。
15. 陳昭儀(2008)。傑出音樂家生涯歷程之研究。特殊教育研究學刊,33(2),113-132。